Robust Cesium Lead Halide Perovskite Microcubes for Frequency Upconversion Lasing

Abstract

FETs), [10,11] memristors, [12,13] and nano lasers [14][15][16] because of their unique optical and electronic characteristics. Recently, much research has been carried on the amplified spontaneous emission (ASE) and lasing of perovskite materials because of their tunable bandgap. For examples, Xing et al. have reported lowtemperature solutionprocessed wavelengthtunable perovskites for lasing, [17] and Xiong et al. have reported nearinfrared nanolasers (Q around 1320) based on organic-inor ganic hybrid perovskite CH 3 NH 3 PbX 3 (X = Cl, Br, I) nanoplatelets. [18] However, regardless of their superior optoelectronic performance, the instability of organicinorganic hybrid perovskites due to their susceptibility for hydrolysis is recog nized as a critical issue for their further practical applications. [19][20][21] Compared to organic-inorganic hybrid perovskites, an allinorganic cesium lead halide perovskite CsPbX 3 (X = Cl, Br, I) has been developed to improve the chemical stability. [22][23][24] In the past several years, allinorganic perovskite nanomaterials CsPbX 3 (X = Cl, Br, I) have found many applications including for amplified spontaneous emission (ASE), lasing, and displays thanks to their excel lent optical performance. [25][26][27][28][29] It is well known that one and twodimensional (2D) crystals, including nanowires, [25,30] nanorods, [31] nanoplates, [30] and microplates [32] are efficient optical gain materials for optical amplification. Moreover, Halide perovskite nanomaterials have recently attracted a lot of attention in the nanoscale laser research field, especially two-photon pumped lasing in halide perovskite nanomaterials has been considered as an ideal alternative strategy to achieve frequency upconversion. However, the poor stability of current organic-inorganic lead halide perovskite materials hinder their further practical applications. Herein, facile solution-processed cesium lead halide perovskite CsPbX 3 (X = Br, I, or Cl) microcubes with low-threshold lasing, high quality, enhanced stability, and excellent wavelength tunability are reported. These as-prepared CsPbX 3 microcubes display excellent structure stability under ambient conditions for several months and they are found to be more robust than their organic-inorganic counterparts. The smooth end facets and wavelength-comparable dimensions make these microcubes promising for high-quality laser cavities in three dimensions. Fabry-Perot lasing is demonstrated in CsPbX 3 microcubes, the process of which is investigated by dynamic emission. In addition, tunable amplified spontaneous emission is achieved with low threshold under both one-and two-photon excitation, which can maintain a stable emission for over 10 hours under continuous intense laser shots in ambient atmosphere. The findings suggest that solution-processed all-inorganic perovskite microcubes can be used as excellent gain medium for frequency upconversion lasers, which would offer a new platform for nonlinear photoelectric devices.

Solution‐Processed Perovskite Microdisk for Coherent Light Emission

“…In CsPbBr 3 NCs, the ASE threshold typically is limited by the surface fast charge carrier trapping and multiparticle Auger recombination . However, the two‐photon pumped threshold of embedded CsPbBr 3 NCs of CsPbBr 3 ‐in‐Cs 4 PbBr 6 CMDs pump power P = 400 µJ cm −2 is comparable with or lower than many other reported two‐photon pumped CsPbBr 3 NCs or microcrystals (Table S3, Supporting Information) . The low threshold indicates the CsPbBr 3 NCs are well passivated by the Cs 4 PbBr 6 matrix and the Auger recombination may also be restricted in such CsPbBr 3 (dot)‐in‐Cs 4 PbBr 6 (huge thick shell) system.…”

Recent Progress in Metal Halide Perovskite Micro‐ and Nanolasers

“…In this section, recent developments of halide perovskite micro‐/nanostructures are discussed according to the structure and morphology dimensionality. The representative works over the past 5 years are summarized in Table 2 and Figure …”

Tunable Halide Perovskites for Miniaturized Solid‐State Laser Applications

“…Hu et al reported the two‐photon pumped FP cavity lasing with stability and wavelength tunability from the facile solution‐processed CsPbX 3 perovskite microcubes. A low lasing threshold (≈439 µJ·cm −2 ), high‐quality factor (Q ≈ 1150), and robust laser stability of over 10 h under continuous intense laser shots in ambient atmosphere were observed (up to 3.6 × 10 7 excitation cycles) …”